Browsing by Author "van de Krol, Roel"
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- ItemThe electronic structure and the formation of polarons in Mo-doped BiVO4 measured by angle-resolved photoemission spectroscopy(London : RSC Publishing, 2019) Mohamed, Mansour; May, Matthias M.; Kanis, Michael; Brützam, Mario; Uecker, Reinhard; van de Krol, Roel; Janowitz, Christoph; Mulazzi, MattiaWe experimentally investigated the electronic structure of Mo-doped BiVO4 high-quality single-crystals with synchrotron radiation-excited angle-resolved photoelectron spectroscopy (ARPES). By photon-energy dependent ARPES, we measured the bulk-derived valence band dispersion along the direction normal to the (010) cleavage plane, while the dispersion along the in-plane directions is obtained by angle-dependent measurements at fixed photon energy. Our data show that the valence band has a width of about 4.75 eV and is composed of many peaks, the two most intense have energies in good agreement with the theoretically calculated ones. A non-dispersive feature is observed in the fundamental gap, which we attribute to quasiparticle excitations coupling electrons and phonons, i.e. polarons. The determination of the polaron peak binding energy and bulk band gap allows to fix the value of the theoretical mixing parameter necessary in hybrid Hartree–Fock calculations to reproduce the experimental data. The attribution of the in-gap peak to polarons is strengthened by our discussion in the context of experimental transport data and ab initio theory.
- ItemProtection Mechanism against Photocorrosion of GaN Photoanodes Provided by NiO Thin Layers(Weinheim : Wiley-VCH, 2020) Kamimura, Jumpei; Budde, Melanie; Bogdanoff, Peter; Tschammer, Carsten; Abdi, Fatwa F.; van de Krol, Roel; Bierwagen, Oliver; Riechert, Henning; Geelhaar, LutzThe photoelectrochemical properties of n-type Ga-polar GaN photoelectrodes covered with NiO layers of different thicknesses in the range 0–20 nm are investigated for aqueous solution. To obtain layers of well-defined thickness and high crystal quality, NiO is grown by plasma-assisted molecular-beam epitaxy. Stability tests reveal that the NiO layers suppress photocorrosion. With increasing NiO thickness, the onset of the photocurrent is shifted to more positive voltages and the photocurrent is reduced, especially for low bias potentials, indicating that hole transfer to the electrolyte interface is hindered by thicker NiO layers. Furthermore, cathodic transient spikes are observed under intermittent illumination, which hints at surface recombination processes. These results are inconsistent with the common explanation of the protection mechanism that the band alignment of GaN/NiO enables efficient hole-injection, thus preventing hole accumulation at the GaN surface that would lead to anodic photocorrosion. Interestingly, the morphology of the etch pits as well as further experiments involving the photodeposition of Ag indicate that photocorrosion of GaN photoanodes is related to reductive processes at threading dislocations. Therefore, it is concluded that the NiO layers block the transfer of photogenerated electrons from GaN to the electrolyte interface, which prevents the cathodic photocorrosion. © 2020 The Authors. Solar RRL published by Wiley-VCH GmbH